Headspace-Solid Phase Microextraction (HS-SPME) was applied to the analysis of volatile compounds of virgin olive oils from southern France (Alpes-Maritimes) and Spain (Reus). Forty one compounds were isolated and characterized by GC-RI and GCMS, representing 85.3-92.8% of the total amount. (E)-Hex-2-enal, the main compound extracted by SPME, characterized the olive oil headspace for all samples. The other compounds identified were mainly hexanal, (Z)-hex-3-enol, (E)-hex-2-enol and hexanol. Changes in the chemical composition of the olive oil headspace were also monitored during storage. The content of (E)-hex-2-enal decreased over several months, and that of the C-6 alcohols and C-5 ketones increased. These compounds can be used as markers for the evaluation of olive oil quality. (C) 2004 Elsevier Ltd. All rights reserved.